The University of Southampton
University of Southampton Institutional Repository

Symmetry-based singlet-triplet excitation in solution nuclear magnetic resonance

Symmetry-based singlet-triplet excitation in solution nuclear magnetic resonance
Symmetry-based singlet-triplet excitation in solution nuclear magnetic resonance

Coupled pairs of spin-1/2 nuclei support one singlet state and three triplet states. In many circumstances, the nuclear singlet order, defined as the difference between the singlet population and the mean of the triplet populations, is a long-lived state that persists for a relatively long time in solution. Various methods have been proposed for generating singlet order, starting from nuclear magnetization. This requires the stimulation of singlet-to-triplet transitions by modulated radiofrequency fields. We show that a recently described pulse sequence, known as PulsePol [Schwartz et al., Sci. Adv., 4, eaat8978 (2018)], is an efficient technique for converting magnetization into long-lived singlet order. We show that the operation of this pulse sequence may be understood by adapting the theory of symmetry-based recoupling sequences in magic-angle-spinning solid-state nuclear magnetic resonance (NMR). The concept of riffling allows PulsePol to be interpreted by using the theory of symmetry-based pulse sequences and explains its robustness. This theory is used to derive a range of new pulse sequences for performing singlet-triplet excitation and conversion in solution NMR. Schemes for further enhancing the robustness of the transformations are demonstrated.

0021-9606
Sabba, Mohamed
bef5e5e8-18b2-43d9-8969-4a9b25bb8691
Wili, Nino
d90cbb1f-1c6b-4b65-99a4-d90ead875b89
Bengs, Christian
cd3282d0-27ad-444f-bcb4-70eeab0029b9
Whipham, James W.
27ba091b-cbc5-40c6-914a-6ab9362c9c2c
Brown, Lynda J.
75aa95fa-5d27-46a7-9dbe-0f465a664f5b
Levitt, Malcolm H.
bcc5a80a-e5c5-4e0e-9a9a-249d036747c3
Sabba, Mohamed
bef5e5e8-18b2-43d9-8969-4a9b25bb8691
Wili, Nino
d90cbb1f-1c6b-4b65-99a4-d90ead875b89
Bengs, Christian
cd3282d0-27ad-444f-bcb4-70eeab0029b9
Whipham, James W.
27ba091b-cbc5-40c6-914a-6ab9362c9c2c
Brown, Lynda J.
75aa95fa-5d27-46a7-9dbe-0f465a664f5b
Levitt, Malcolm H.
bcc5a80a-e5c5-4e0e-9a9a-249d036747c3

Sabba, Mohamed, Wili, Nino, Bengs, Christian, Whipham, James W., Brown, Lynda J. and Levitt, Malcolm H. (2022) Symmetry-based singlet-triplet excitation in solution nuclear magnetic resonance. Journal of Chemical Physics, 157 (13), [134302]. (doi:10.1063/5.0103122).

Record type: Article

Abstract

Coupled pairs of spin-1/2 nuclei support one singlet state and three triplet states. In many circumstances, the nuclear singlet order, defined as the difference between the singlet population and the mean of the triplet populations, is a long-lived state that persists for a relatively long time in solution. Various methods have been proposed for generating singlet order, starting from nuclear magnetization. This requires the stimulation of singlet-to-triplet transitions by modulated radiofrequency fields. We show that a recently described pulse sequence, known as PulsePol [Schwartz et al., Sci. Adv., 4, eaat8978 (2018)], is an efficient technique for converting magnetization into long-lived singlet order. We show that the operation of this pulse sequence may be understood by adapting the theory of symmetry-based recoupling sequences in magic-angle-spinning solid-state nuclear magnetic resonance (NMR). The concept of riffling allows PulsePol to be interpreted by using the theory of symmetry-based pulse sequences and explains its robustness. This theory is used to derive a range of new pulse sequences for performing singlet-triplet excitation and conversion in solution NMR. Schemes for further enhancing the robustness of the transformations are demonstrated.

Text
JCP22-AR-02014 (2) - Accepted Manuscript
Available under License Creative Commons Attribution.
Download (7MB)
Text
5.0103122 - Version of Record
Available under License Creative Commons Attribution.
Download (7MB)

More information

Accepted/In Press date: 24 August 2022
e-pub ahead of print date: 4 October 2022
Published date: 7 October 2022
Additional Information: Funding Information: We acknowledge funding received by the European Research Council (Grant No. 786707-FunMagResBeacons) and EPSRC-UK (Grant Nos. EP/P009980/1, EP/P030491/1, and EP/V055593/1). We thank Sami Jannin, Quentin Stern, Chloé Gioiosa, Olivier Cala, Lau-rynas Dagys, Stuart J. Elliott, and Maria Concistré for help and discussions. Publisher Copyright: © 2022 Author(s).

Identifiers

Local EPrints ID: 472429
URI: http://eprints.soton.ac.uk/id/eprint/472429
ISSN: 0021-9606
PURE UUID: 5ec3869e-dda6-4a9e-b181-59acbc7d29a7
ORCID for Mohamed Sabba: ORCID iD orcid.org/0000-0003-2707-1821
ORCID for Christian Bengs: ORCID iD orcid.org/0000-0002-0196-7817
ORCID for Lynda J. Brown: ORCID iD orcid.org/0000-0002-5678-0814
ORCID for Malcolm H. Levitt: ORCID iD orcid.org/0000-0001-9878-1180

Catalogue record

Date deposited: 05 Dec 2022 17:50
Last modified: 06 Jun 2024 02:10

Export record

Altmetrics

Contributors

Author: Mohamed Sabba ORCID iD
Author: Nino Wili
Author: Christian Bengs ORCID iD
Author: James W. Whipham
Author: Lynda J. Brown ORCID iD

Download statistics

Downloads from ePrints over the past year. Other digital versions may also be available to download e.g. from the publisher's website.

View more statistics

Atom RSS 1.0 RSS 2.0

Contact ePrints Soton: eprints@soton.ac.uk

ePrints Soton supports OAI 2.0 with a base URL of http://eprints.soton.ac.uk/cgi/oai2

This repository has been built using EPrints software, developed at the University of Southampton, but available to everyone to use.

We use cookies to ensure that we give you the best experience on our website. If you continue without changing your settings, we will assume that you are happy to receive cookies on the University of Southampton website.

×